Achieving Tunable Cold/Warm White‑Light Emission in a Single Perovskite Material with Near‑Unity Photoluminescence Quantum Yield

Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications.This paper reports a novel zero-dimensional perovskite,Rb_(4)CdCl_(6):Sn^(2+),Mn^(2+),which demonstrates exceptional white-light properties including adjustable correlated color temperature,high color rendering index of up to 85,and near-unity photoluminescence quantum yield of 99%.Using a co-doping strategy involving Sn^(2+)and Mn^(2+),cyan-orange dual-band emission with complementary spectral ranges is activated by the self-trapped excitons and d-d transitions of the Sn^(2+)and Mn^(2+)centers in the Rb_(4)CdCl_(6)host,respectively.Intriguingly,although Mn^(2+)ions doped in Rb_(4)CdCl_(6)are difficult to excite,efficient Mn^(2+)emission can be realized through an ultra-high-efficient energy transfer between Sn^(2+)and Mn^(2+)via the formation of adjacent exchange-coupled Sn–Mn pairs.Benefiting from this efficient Dexter energy transfer process,the dual emission shares the same optimal excitation wavelengths of the Sn^(2+)centers and suppresses the non-radiative vibration relaxation significantly.Moreover,the relative intensities of the dual-emission components can be modulated flexibly by adjusting the fraction of the Sn^(2+)ions to the Sn–Mn pairs.This co-doping approach involving short-range energy transfer represents a promising avenue for achieving high-quality white light within a single material.

Controllable one-step doping synthesis for the white-light emission of cesium copper iodide perovskites

In this paper, a controllable one-step doping method has been successfully adopted in the cesium copper iodide perovskite’s luminescence, a high-quality white-light emission with Commission Internationale de l’Eclairage(CIE) coordinates of(0.3397, 0.3325), and a color rendering index(CRI) reaching up to 90 was realized in a convenient way. Through adding impurities into the Cs_(3)Cu_(2)I_(5) system, high efficiency and stable CsCu_(2)I_(3) was synthesized, and the coexistence of varied high luminescence phases realized the white lighting.Strikingly, blue-emitting Cs_(3)Cu_(2)I_(5) and yellow-emitting CsCu_(2)I_(3) could coexist, and their respective luminescence was not interacted in the compound, which was beneficial for acquiring a single emission and highly efficient white lighting. This work carried out a deep exploration of the Cu-based metal halides, and would be favorable to the applications of lead-free perovskites.

Generation of ultrafast radially polarized pulses through chirp-assisted femtosecond optical parametric amplification

Radially polarized beams characterized by an axially symmetric polarization distribution can be sharply focused to produce strong longitudinal fields in the vicinity.Future applications of these beams will be facilitated by the availability of higher powers and shorter durations.Currently,the ultrafast radially polarized pulse is typically generated via wavefront reconstruction from conventional linearly polarized states.Achievable pulse duration and intensity limits are strictly dependent on extra-cavity optics.Herein,a chirp-assisted near-degenerate type-II parametric process is presented as a pulse-energy-scalable method of accessing ultrafast radially polarized pulses.In a proof-of-principle experiment,the broadband gain balance between the orthogonally polarized signal components was realized via controlling the chirp of the pump pulse.Through an analogous pulseduration transfer effect,the radially polarized signal inherited the temporal and spectral characteristics of the pump pulse and maintained the radial polarization state of each frequency component of the signal.With a shorter pump pulse,the generation of few-cycle radially polarized pulses should be achievable,which may facilitate a wide range of ultrafast applications such as vacuum electron acceleration and high-harmonic generation.

Efficient idler broadening via oppositely dual-chirped difference frequency generation

Dual-chirped difference frequency generation(DFG)is an advantageous technique for generating the broadband midinfrared(IR)idler wave,which is inaccessible by a population-inversion-based laser system.In principle,the generated idler wave may even suffer a spectrum broadening compared with the driving pulsed lasers if the pump and signal waves are oppositely chirped.However,broadband phase-matching is always the determining factor for the resulting efficiency and the bandwidth of the generated idler wave.In this study,specific to an oppositely dual-chirped DFG scheme,we derive the precondition to realize broadband frequency conversion,wherein a negative(1/υp-1/υi)/(1/υs-1/υi),in terms of the correlation coefficient of the group velocity(σ),is necessary.However,most birefringence bulk crystals can only provide the required material dispersions in limited spectral regions.We show that the periodically poled lithium niobate crystal that satisfies an inactive Type-II(eo-o)quasi-phase-matching condition has a stable negativeσand exerts the expected broadband gain characteristic across an ultra-broad idler spectral region(1.7-4.0µm).Finally,we propose and numerically verify a promising DFG configuration to construct a tunable mid-IR spectrum broader based on the broadband phase-matched oppositely dual-chirped DFG scheme.

Frequency-domain parametric downconversion for efficient broadened idler generation

An opposite-chirped frequency-domain optical parametric amplification(OC-FOPA) design is demonstrated and numerically verified. This scheme combines both an ultrabroad seeding generation and the subsequent effective amplification in one single optical parametric amplification stage. Based on a slightly asymmetrical 4-f optical system, the spectral contents of both pump and signal waves are spectrally dispersed with opposite spatial chirps,to broaden the initial idler seeding. Via a properly designed fan-out periodically poled LiNbO_3 chip, nearly perfect quasi phase matching can be realized across the full spectrum, whereby each individual spectral pair precisely maps to its required grating period. Full-dimensional simulations based on commercial ~110 fs(FWHM) nearinfrared(near-IR) lasers at 790 and 1030 nm are quantitatively discussed, and few-cycle mid-IR laser pulses(~60 fs at 3.4 μm) plus a high conversion efficiency exceeding 50% are theoretically predicted. By means of a high-power pump source, the OC-FOPA scheme can be also applied to directly produce high-intensity carrier-envelope-phase-stabilized mid-IR idler pulses.